Zitieren Sie bitte immer diesen URN: urn:nbn:de:kobv:b43-559310
The Mechanochemical Excitation of Crystalline LiN3
- Mechanochemical reactions are driven by the direct absorption of mechanical energy by a solid (often crystalline) material. Understanding how this energy is absorbed and ultimately causes a chemical transformation is essential for understanding the elementary stages of mechanochemical transformations. Using as a model system the energetic material LiN3 we here consider how vibrational energy flows through the crystal structure. By considering the compression response of the crystalline material we identify the partitioning of energy into an initial vibrational excitation. Subsequent energy flow is based on concepts of phonon–phonon scattering, which we calculate within a quasi-equilibrium model facilitated by phonon scattering data obtained from Density Functional Theory (DFT). Using this model we demonstrate how the moments (picoseconds) immediately following mechanical impact lead to significant thermal excitation of crystalline LiN3, sufficient to drive marked changes in itsMechanochemical reactions are driven by the direct absorption of mechanical energy by a solid (often crystalline) material. Understanding how this energy is absorbed and ultimately causes a chemical transformation is essential for understanding the elementary stages of mechanochemical transformations. Using as a model system the energetic material LiN3 we here consider how vibrational energy flows through the crystal structure. By considering the compression response of the crystalline material we identify the partitioning of energy into an initial vibrational excitation. Subsequent energy flow is based on concepts of phonon–phonon scattering, which we calculate within a quasi-equilibrium model facilitated by phonon scattering data obtained from Density Functional Theory (DFT). Using this model we demonstrate how the moments (picoseconds) immediately following mechanical impact lead to significant thermal excitation of crystalline LiN3, sufficient to drive marked changes in its electronic structure and hence chemical reactivity. This work paves the way towards an ab initio approach to studying elementary processes in mechanochemical reactions involving crystalline solids.…
Autor*innen: | Adam MichalchukORCiD |
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Dokumenttyp: | Zeitschriftenartikel |
Veröffentlichungsform: | Verlagsliteratur |
Sprache: | Englisch |
Titel des übergeordneten Werkes (Englisch): | Faraday Discussions |
Jahr der Erstveröffentlichung: | 2022 |
Organisationseinheit der BAM: | 6 Materialchemie |
6 Materialchemie / 6.0 Abteilungsleitung und andere | |
6 Materialchemie / 6.3 Strukturanalytik | |
Veröffentlichende Institution: | Bundesanstalt für Materialforschung und -prüfung (BAM) |
Verlag: | Royal Society of Chemistry |
Erste Seite: | 1 |
Letzte Seite: | 20 |
DDC-Klassifikation: | Technik, Medizin, angewandte Wissenschaften / Ingenieurwissenschaften / Ingenieurwissenschaften und zugeordnete Tätigkeiten |
Technik, Medizin, angewandte Wissenschaften / Ingenieurwissenschaften / Ingenieurbau | |
Freie Schlagwörter: | Ab initio simulation; DFT; Energetic materials; Mechanochemistry |
Themenfelder/Aktivitätsfelder der BAM: | Infrastruktur |
Infrastruktur / Security | |
Material | |
Material / Materialdesign | |
DOI: | 10.1039/d2fd00112h |
URN: | urn:nbn:de:kobv:b43-559310 |
Verfügbarkeit des Dokuments: | Datei für die Öffentlichkeit verfügbar ("Open Access") |
Lizenz (Deutsch): | Creative Commons - CC BY-NC - Namensnennung - Nicht kommerziell 4.0 International |
Datum der Freischaltung: | 10.10.2022 |
Referierte Publikation: | Ja |
Datum der Eintragung als referierte Publikation: | 10.10.2022 |
Schriftenreihen ohne Nummerierung: | Wissenschaftliche Artikel der BAM |